Efficient molecular dissociation by a chirped ultrashort infrared laser pulse

Dissociation probabilities and populations of excited vibrational states are calculated numerically for interaction of a Morse oscillator with a chirped, ultrashort (${\mathit{t}}_{\mathit{p}}$<${10}^{\mathrm{-}11}$ sec), intense laser pulse. It is shown that if the pulse frequency ω(t) decreases at a specific rate adapted to the molecular anharmonicity, the dissociation probability is many orders of magnitude higher than for a monochromatic pulse of the same intensity. Such pulses should be useful for more efficient multiphoton dissociation of molecular bonds.